Spontaneous, Catalyst-Free Co-Polymerization of Ionic Liquids With CO₂ Toward Polycarbonate

The conversion of carbon dioxide (CO₂) into value-added polymer is a cornerstone of sustainable chemistry, yet current strategies typically require high pressures, metal catalysts, and yield materials with limited functionality. Herein, we report a spontaneous, catalyst-free polymerization that directly converts CO₂ and hydroxyl-functionalized ionic liquids (ILs) into multifunctional ionic polycarbonates under ambient conditions (0.1 MPa, 60°C). Mechanism studies, combining spectroscopic analysis and density functional calculations, elucidate a synergistic process wherein IL cations function as CO₂ concentrators, while OH^- anions drive the polymerization via a bicarbonate-mediated nucleophilic pathway. This approach yields a well-defined ionic polycarbonate that uniquely integrates high ionic conductivity (>10^{- 4} S·m^{- 1}), dual-wavelength fluorescence, broad-spectrum antibacterial activity (>99% inhibition against E. coli and S. aureus), and performance as a multifunctional adhesive enhancer with self-monitoring capability. Furthermore, these polymers undergo complete degradation into monomeric constituents, establishing a closed-loop monomer-polymer-monomer lifecycle. This work provides a paradigm for sustainable CO₂ valorization into advanced multifunctional materials, with immediate potential in smart adhesives, wearable electronics, and information encryption.